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CN102903591A - Ultrafast lens-free coherent electron diffraction imaging method and device - Google Patents

Ultrafast lens-free coherent electron diffraction imaging method and device Download PDF

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CN102903591A
CN102903591A CN2012103857012A CN201210385701A CN102903591A CN 102903591 A CN102903591 A CN 102903591A CN 2012103857012 A CN2012103857012 A CN 2012103857012A CN 201210385701 A CN201210385701 A CN 201210385701A CN 102903591 A CN102903591 A CN 102903591A
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陈洁
王西杰
陈明伟
朱溢眉
朱鹏飞
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Shanghai Jiao Tong University
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Abstract

本发明公开了一种超快无透镜相干电子衍射成像方法及装置,通过与过程激发源(如飞秒激光脉冲)精确同步的电子脉冲和无透镜相干衍射成像技术相结合,分析被衍射的相干电子脉冲的强度分布,反演计算确定电子散射相位,实现三维瞬态原子尺度的结构和形貌重构,解决传统的电子显微成像方法不具有高时间分辨能力或目前的超快电子成像时间和空间分辨率受限的技术困境。

The invention discloses an ultrafast lensless coherent electron diffraction imaging method and device, which can analyze the diffracted coherent Intensity distribution of electron pulses, inversion calculation to determine electron scattering phase, realize three-dimensional transient atomic scale structure and shape reconstruction, solve the problem that traditional electron microscopy imaging methods do not have high time resolution or the current ultrafast electron imaging time and the technical dilemma of limited spatial resolution.

Description

超快无透镜相干电子衍射成像方法及装置Ultrafast lensless coherent electron diffraction imaging method and device

技术领域 technical field

本发明涉及时间分辨的电子显微成像,特别是一种具有优于1皮秒时间分辨率和优于1纳米空间分辨率的超快无透镜相干电子衍射成像方法及其可能的相应装置。 The present invention relates to time-resolved electron microscopy imaging, in particular to an ultrafast lensless coherent electron diffraction imaging method with a temporal resolution better than 1 picosecond and a spatial resolution better than 1 nanometer and a possible corresponding device.

背景技术 Background technique

本发明涉及的背景技术分为两方面; The background technology involved in the present invention is divided into two aspects;

一、电子显微镜的时间和空间分辨率问题:传统的电子显微成像通过提高电子加速电压、使用电磁透镜、提高电子源的品质三个主要方向,其空间分辨率的提高已经几近极限。由于传统的电子显微成像一般是时间累积的形貌成像,无法对物理、化学、生物等各领域中的过程进行高时间分辨成像。因此,在传统的电子显微成像技术中引入时间分辨能力,是当今世界科技发展的前沿。已有的时间分辨电子成像系统中,比较典型的有美国加州理工学院(Caltech)Zewail研究组的超快电子显微镜(ultrafast electron microscopy, UEM),美国劳伦斯·利弗莫尔国家实验室(LLNL)Campbell研究组的动态透射电子显微镜(dynamic transmission electron microscope, DTEM)。 1. The temporal and spatial resolution of the electron microscope: The traditional electron microscopic imaging has three main directions: increasing the electron accelerating voltage, using an electromagnetic lens, and improving the quality of the electron source, and its spatial resolution has been improved to the limit. Since traditional electron microscopic imaging is generally time-accumulated topography imaging, it is impossible to perform high-time-resolved imaging of processes in various fields such as physics, chemistry, and biology. Therefore, the introduction of time-resolution capability into traditional electron microscopy imaging technology is at the forefront of technological development in the world today. Among the existing time-resolved electronic imaging systems, the typical ultrafast electron microscopy (UEM) of the Zewail research group at the California Institute of Technology (Caltech) and the Lawrence Livermore National Laboratory (LLNL) The dynamic transmission electron microscope (DTEM) of Campbell's research group.

在这些时间分辨电子成像系统中,从衍射空间(即倒空间)到实空间的电子成像是通过电磁物镜主导的傅里叶变换实现的,由于电子经过样品后使用电磁物镜进行成像,损失了电子的相位信息,因此这些系统在空间分辨率和时间分辨率的提高上都受限。一方面,电子束的电磁透镜成像的空间分辨率提高有两个重大技术困难:一是要求透镜的像差极小,否则相位误差将引入到衍射波中,无法获得清晰像,对于电子透镜成像和X射线波带片成像,实现这一点极端困难;二是整个实验装置必须足够稳定,从而位于衍射平面边缘的大角度电子仍然可以在像平面相干干涉。所以,即使通过复杂的像差矫正,一般电子透镜的可用角度范围也仅仅在1-2度,这种动量空间(换句话说,透镜可以接纳入射电子束的最大散射范围)的限制严重地影响了空间分辨率。另一方面,由于电子作为带电粒子会相互排斥,经过电磁透镜的长距离飞行过程中,电子脉冲宽度会展宽,从而导致时间分辨率降低。 In these time-resolved electronic imaging systems, electron imaging from diffraction space (i.e., inverted space) to real space is realized by Fourier transform dominated by electromagnetic objective lens, since the electrons pass through the sample and use electromagnetic objective lens for imaging, the loss of electron Therefore, these systems are limited in the improvement of spatial resolution and temporal resolution. On the one hand, there are two major technical difficulties in improving the spatial resolution of electron beam electromagnetic lens imaging: one is that the aberration of the lens is required to be extremely small, otherwise the phase error will be introduced into the diffracted wave, and a clear image cannot be obtained. It is extremely difficult to achieve this with X-ray zone plate imaging; second, the entire experimental device must be stable enough so that large-angle electrons located at the edge of the diffraction plane can still interfere coherently at the image plane. Therefore, even with complex aberration correction, the usable angular range of general electron lenses is only 1-2 degrees. This limitation of momentum space (in other words, the maximum scattering range that the lens can accept the incident electron beam) seriously affects the spatial resolution. On the other hand, since electrons repel each other as charged particles, the pulse width of electrons will be broadened during the long-distance flight through the electromagnetic lens, resulting in a decrease in time resolution.

二、相干无透镜衍射成像:它借助于理论方法和计算机算法解决周期和非周期结构样品中衍射的相位问题,在X射线领域被称为相干X射线衍射成像(coherent x-ray diffractive imaging, CXDI)。人们很早就意识到可见光领域的相位问题,瑞利在给迈克耳逊的一封信中曾经评论说,如果没有数据对称性的相关信息,干涉中的相位问题是无法解决的。相位问题成功解决归功于D. Sayre,他在1952年指出应该考虑Shannon的取样理论和布拉格定律间的关系[Acta Crystallogr. 5, 843(1952)]。其后,Gerchberg和Saxton第一次编写出了恢复相位的算法[Optik 35,237(1972)]。这种算法常被称为hybrid input–output (HIO) algorithm [Appl. Opt. 21,2758(1982)]:对一个原函数在实空间和傅里叶空间反复迭代,每一次迭代都对实空间或者傅里叶空间加边界条件。此领域在1990年前后开始得到快速发展,其中苗建伟等人1999年首次在软x射线波段进行了实验验证[Nature 400,342(1999)];随后左建明等人2003年率先发表了电子相干无透镜衍射成像的实验研究成果[Science 300, 1419(2003)], 2008年朱溢眉等人提出“位置敏感衍射成像”(position-sensitive diffractive imaging, PSDI)用于电子的相干无透镜衍射成像。在过去的20年间,这项技术从结晶学外延到对非晶样品的高分辨率成像,并得到广泛应用[Adv. Phys. 59, 1 (2010)]。 2. Coherent lensless diffraction imaging: It uses theoretical methods and computer algorithms to solve the phase problem of diffraction in samples with periodic and non-periodic structures. It is called coherent x-ray diffractive imaging (CXDI) in the X-ray field. ). Phase problems in the visible domain have been recognized very early, and Rayleigh once commented in a letter to Michelson that phase problems in interferometry cannot be solved without relevant information about the symmetry of the data. The successful solution of the phase problem is attributed to D. Sayre, who pointed out in 1952 that the relationship between Shannon's sampling theory and Bragg's law should be considered [Acta Crystallogr. 5, 843(1952)]. Subsequently, Gerchberg and Saxton wrote the algorithm for recovering the phase for the first time [Optik 35, 237 (1972)]. This algorithm is often called the hybrid input–output (HIO) algorithm [Appl. Opt. 21, 2758 (1982)]: iterates an original function in real space and Fourier space repeatedly, and each iteration performs real space Or Fourier space plus boundary conditions. This field began to develop rapidly around 1990. In 1999, Miao Jianwei et al. carried out experimental verification in the soft X-ray band for the first time [Nature 400,342(1999)]; The experimental research results of lens diffraction imaging [Science 300, 1419 (2003)], in 2008, Zhu Yimei and others proposed "position-sensitive diffractive imaging" (PSDI) for coherent lensless diffraction imaging of electrons. In the past 20 years, this technique has been widely used from crystallographic epitaxy to high-resolution imaging of amorphous samples [Adv. Phys. 59, 1 (2010)].

相干电子衍射成像的基本原理是利用拟合电子衍射的衍射强度,通过逆向演算找回由于缺少物镜所丢失的样品相位信息。基于电子衍射的相干无透镜成像,对装置的高稳定性的要求和对入射束的能散要求相对放松。相干成像无需物镜,直接利用光敏薄膜或者电荷耦合元件(CCD)探测器记录衍射图样的强度。衍射成像的优势在于干涉条件是否满足仅仅决定于样品内部本身的散射,不要求电子束流在传输系统中长距离漂移后再干涉。然而与传统电子显微成像类似,该方法还不具有时间分辨能力。 The basic principle of coherent electron diffraction imaging is to use the diffraction intensity of fitting electron diffraction to retrieve the phase information of the sample lost due to the lack of objective lens through reverse calculation. For coherent lensless imaging based on electron diffraction, the requirements for high stability of the device and energy dispersion of the incident beam are relatively relaxed. Coherent imaging does not require an objective lens, and directly uses a photosensitive film or a charge-coupled device (CCD) detector to record the intensity of the diffraction pattern. The advantage of diffraction imaging is that whether the interference conditions are satisfied is only determined by the scattering inside the sample itself, and does not require the electron beam to interfere after long-distance drift in the transmission system. However, similar to traditional electron microscopy imaging, this method is not yet time-resolved.

因此传统的电子显微成像技术,主要存在如下技术问题: Therefore, the traditional electron microscopic imaging technology mainly has the following technical problems:

1.      无时间分辨能力或时间分辨率受限。 1. No time resolution capability or limited time resolution.

2.      空间分辨率低:实空间像的空间分辨率受物镜的质量(如像差和色差等)制约,通过采用高质量的电磁物镜提高空间分辨率的成本高。 2. Low spatial resolution: The spatial resolution of real space images is restricted by the quality of the objective lens (such as aberration and chromatic aberration, etc.), and the cost of improving spatial resolution by using high-quality electromagnetic objective lenses is high.

3.      提高时间分辨率的成本高:尽管可以通过采用兆电子伏特电子脉冲来抑制电子脉冲飞行过程中的展宽问题,从而提高时间分辨率,但电磁物镜的成本与聚焦电子束的能量一般成正比关系(大约人民币40元每电子伏特),将极大程度地增加成本。 3. High cost of improving time resolution: Although time resolution can be improved by using MeV electron pulses to suppress the problem of electron pulse broadening during flight, the cost of electromagnetic objectives is generally proportional to the energy of the focused electron beam ( About RMB 40 per electron volt), which will greatly increase the cost.

发明内容 Contents of the invention

本发明的目的在于克服上述现有技术的不足,提供一种超快无透镜相干电子衍射成像方法及装置。超快指相对于传统的电子显微成像技术,具有高时间分辨率,特指可实现优于1皮秒的时间分辨率。它通过与过程激发源(如飞秒激光脉冲)精确同步的电子脉冲和无透镜相干衍射成像技术相结合,分析被衍射的相干电子脉冲的强度分布,反演计算确定电子散射相位,实现三维瞬态原子尺度的结构和形貌重构,解决传统的电子显微成像方法不具有高时间分辨能力或目前的超快电子成像时间和空间分辨率受限的技术困境。 The object of the present invention is to overcome the shortcomings of the above-mentioned prior art, and provide an ultrafast lensless coherent electron diffraction imaging method and device. Compared with traditional electron microscopic imaging technology, ultrafast means that it has high time resolution, especially that it can achieve a time resolution better than 1 picosecond. It combines electron pulses precisely synchronized with process excitation sources (such as femtosecond laser pulses) and lens-free coherent diffraction imaging technology to analyze the intensity distribution of diffracted coherent electron pulses, determine the electron scattering phase through inversion calculation, and realize three-dimensional instantaneous The structure and shape reconstruction at the atomic scale solves the technical dilemma that the traditional electron microscopy imaging method does not have high time resolution or the current ultrafast electron imaging is limited in time and space resolution.

本发明的技术解决方案如下: Technical solution of the present invention is as follows:

一种超快无透镜相干电子衍射成像方法,其特点在于:该方法结合泵浦-探测技术和无透镜相干电子衍射成像,以同时实现超高时间分辨和超高空间分辨的瞬态成像;该方法采用与过程激发脉冲精确同步的高亮度相干电子脉冲作为探测源;探测电子经过样品后不经过任何电子光学系统(即电磁透镜),直接由探测系统收集相干电子衍射成像图样,从而保持电子的散射相位信息;该方法从所述的相干电子衍射成像通过数据处理和三维重构系统利用现有的反演计算方法计算电子的散射相位信息,实现三维瞬态原子尺度的结构和形貌重构。 An ultra-fast lensless coherent electron diffraction imaging method, which is characterized in that: the method combines pump-probe technology and lensless coherent electron diffraction imaging to simultaneously realize transient imaging with ultra-high time resolution and ultra-high spatial resolution; The method uses a high-brightness coherent electron pulse precisely synchronized with the process excitation pulse as the detection source; after the detection electron passes through the sample, it does not pass through any electron optical system (ie, electromagnetic lens), and the coherent electron diffraction imaging pattern is directly collected by the detection system, thereby maintaining the electron's Scattering phase information; this method calculates the scattering phase information of electrons from the coherent electron diffraction imaging through data processing and 3D reconstruction system using the existing inversion calculation method, and realizes the structure and shape reconstruction of the three-dimensional transient atomic scale .

实施上述超快无透镜相干电子衍射成像方法的超快无透镜相干电子衍射成像装置,由过程激发源、脉冲电子系统、脉冲电子控制系统、样品、探测系统、数据处理和三维重构系统和高真空样品靶室组成,上述元部件的功能和位置关系如下: The ultrafast lensless coherent electron diffraction imaging device implementing the above ultrafast lensless coherent electron diffraction imaging method consists of a process excitation source, a pulse electronic system, a pulse electronic control system, a sample, a detection system, a data processing and three-dimensional reconstruction system and high The composition of the vacuum sample target chamber, the functions and positions of the above components are as follows:

所述的脉冲电子系统、脉冲电子控制系统、样品和探测系统置于所述的高真空样品靶室内,样品置于高真空样品靶室内的五维调整架上,其中所述的脉冲电子系统由脉冲电子源及其加速、整形元件组成;所述的过程激发源产生过程激发脉冲,输入所述的高真空样品靶室激发位于所述的五维调整架上的样品。 The pulse electronic system, pulse electronic control system, sample and detection system are placed in the high vacuum sample target chamber, and the sample is placed on the five-dimensional adjustment frame in the high vacuum sample target chamber, wherein the pulse electronic system consists of The pulse electron source and its acceleration and shaping components are composed; the process excitation source generates a process excitation pulse, which is input into the high vacuum sample target chamber to excite the sample on the five-dimensional adjustment frame.

所述的脉冲电子源产生与所述的过程激发脉冲精确同步的电子脉冲,该脉冲电子经过加速、整形成为高亮度相干的脉冲电子束,其中空间相干长度优于50纳米,时间相干长度优于50纳米;经过所述的脉冲电子控制系统聚焦照射在处于高真空样品靶室内的被过程激发脉冲激发的样品区域,被所述的样品衍射后,形成一系列相互耦合的、或者相互重叠的衍射图样;该衍射图样由所述的探测系统接收,包括布拉格衍射峰以及布拉格峰间的干涉信息;输入所述的数据处理和三维重构系统,通过在线快速傅里叶方法,从衍射图样中找回相位。 The pulsed electron source generates electron pulses that are precisely synchronized with the process excitation pulses, and the pulsed electrons are accelerated and shaped into high-brightness coherent pulsed electron beams, wherein the spatial coherence length is better than 50 nanometers, and the temporal coherence length is better than 50 nanometers. 50 nanometers; after the pulse electronic control system is focused and irradiated on the sample area excited by the process excitation pulse in the high-vacuum sample target chamber, after being diffracted by the sample, a series of mutually coupled or overlapping diffractions are formed pattern; the diffraction pattern is received by the detection system, including Bragg diffraction peaks and interference information between Bragg peaks; input to the data processing and three-dimensional reconstruction system, through the online fast Fourier method, from the diffraction pattern to find back phase.

所述的过程激发源包括飞秒激光光源、分束镜、由第一激光伺服反射镜、第二激光伺服反射镜和第一平移台构成的第一可变光路延迟调节系统、第三激光伺服反射镜、光参量放大激光转化系统、第四激光伺服反射镜、聚焦透镜构成。 The process excitation source includes a femtosecond laser light source, a beam splitter, a first variable optical path delay adjustment system composed of a first laser servo mirror, a second laser servo mirror and a first translation stage, a third laser servo It consists of a reflector, an optical parametric amplification laser conversion system, a fourth laser servo reflector, and a focusing lens.

所述的脉冲电子系统由高真空样品靶室外的第五激光伺服反射镜、由第六激光伺服反射镜、第七激光伺服反射镜和第二平移台构成的第二光路延迟调节系统、第八激光伺服反射镜、飞秒激光三倍频装置、紫外聚焦透镜和高真空样品靶室内的金属膜和多级微波加速器构成。 The pulsed electronic system consists of the fifth laser servo mirror outside the high-vacuum sample target chamber, the second optical path delay adjustment system composed of the sixth laser servo mirror, the seventh laser servo mirror and the second translation stage, and the eighth laser servo mirror. It consists of a laser servo mirror, a femtosecond laser triple frequency device, an ultraviolet focusing lens, a metal film in a high-vacuum sample target chamber, and a multi-stage microwave accelerator.

所述的脉冲电子控制系统由位于高真空样品靶室内依次的第一偏转板、第二偏转板、由第一电磁透镜、第一孔径、第二电磁透镜和第二孔径构成。 The pulse electronic control system consists of a first deflection plate, a second deflection plate, a first electromagnetic lens, a first aperture, a second electromagnetic lens and a second aperture located in the high vacuum sample target chamber.

沿所述的飞秒激光光源的激光前进方向是所述的分束镜,该分束镜将飞秒激光光源输出的飞秒激光脉冲分为反射光束和透射光束;沿所述的反射光束的前进方向依次经所述的第一激光伺服反射镜、第二激光伺服反射镜、第三激光伺服反射镜、光参量放大激光转化系统、第四激光伺服反射镜反射,经所述的聚焦透镜聚焦后,穿过所述的高真空样品靶室照射位于五轴样品调节架上的样品;沿所述的透射光束的前进方向依次经过所述的第五激光伺服反射镜、第六激光伺服反射镜、第七激光伺服反射镜、第八激光伺服反射镜、飞秒激光三倍频装置和紫外聚焦透镜聚焦后转化为266nm激光脉冲。 Along the laser advance direction of the femtosecond laser source is the beam splitter, which divides the femtosecond laser pulse output by the femtosecond laser source into a reflected beam and a transmitted beam; along the direction of the reflected beam The forward direction is sequentially reflected by the first laser servo mirror, the second laser servo mirror, the third laser servo mirror, the optical parameter amplification laser conversion system, and the fourth laser servo mirror, and then focused by the focusing lens Finally, pass through the high-vacuum sample target chamber to irradiate the sample on the five-axis sample adjustment frame; pass through the fifth laser servo mirror and the sixth laser servo mirror in sequence along the forward direction of the transmitted light beam , the seventh laser servo mirror, the eighth laser servo mirror, the femtosecond laser triple frequency device and the ultraviolet focusing lens are converted into 266nm laser pulses after focusing.

所述的266nm激光脉冲照射位于所述高真空样品靶室内的金属膜,并通过光电效应产生脉冲电子,该电子脉冲经多级微波加速器、第一偏转板、第二偏转板、由第一电磁透镜、第一孔径、第二电磁透镜、第二孔径构成的电子聚焦准直系统后,形成约50纳米或更小的相干电子斑,照射在所述的样品区域内,被衍射形成的布拉格衍射峰和布拉格峰间干涉信息的衍射图样,该衍射图样由所述的探测系统接收,通过所述的数据处理和三维重构系统进行数据处理,利用“位置敏感衍射成像”(PSDI)技术,解析出样品的散射相位信息。 The 266nm laser pulse irradiates the metal film located in the high-vacuum sample target chamber, and generates pulsed electrons through the photoelectric effect. After the electronic focusing and collimating system composed of the lens, the first aperture, the second electromagnetic lens and the second aperture, a coherent electron spot of about 50 nanometers or smaller is formed, which is irradiated in the sample area, and the Bragg diffraction formed by diffraction The diffraction pattern of the interference information between the peak and the Bragg peak, the diffraction pattern is received by the detection system, the data is processed by the data processing and three-dimensional reconstruction system, and the "position-sensitive diffraction imaging" (PSDI) technology is used to analyze The scattering phase information of the sample is obtained.

所述的过程激发脉冲和所述的电子脉冲通过泵浦-探测技术精确同步。 The process excitation pulses and the electron pulses are precisely synchronized by pump-probe technology.

所述的五轴样品调节架具有上下、前后、左右、旋转和倾斜调整姿态。 The five-axis sample adjustment rack has up and down, front and rear, left and right, rotation and tilt adjustment postures.

所述的第一激光伺服反射镜和第二激光伺服反射镜设置于第一平移台上构成的第一可变光路延迟调节系统,所述的第六激光伺服反射镜和第七激光伺服反射镜设置于第二平移台上构成的第二光路延迟调节系统。 The first variable optical path delay adjustment system formed by the first laser servo mirror and the second laser servo mirror being arranged on the first translation stage, the sixth laser servo mirror and the seventh laser servo mirror The second optical path delay adjustment system formed on the second translation stage.

本发明技术解决方案的原理: The principle of technical solution of the present invention:

1.      解决无时间分辨能力或时间分辨率受限问题:采用电子脉冲,特别是可以采用兆电子伏特飞秒电子脉冲,该电子脉冲与过程激发源(如飞秒激光)精确同步。 1. Solve the problem of no time resolution capability or limited time resolution: use electron pulses, especially MeV femtosecond electron pulses, which are precisely synchronized with the process excitation source (such as femtosecond laser).

2.      解决空间分辨率受物镜的质量制约问题:采用无透镜相干电子衍射成像,不使用物镜(即散焦电磁透镜),且缩短电子飞行距离。 2. Solve the problem that the spatial resolution is limited by the quality of the objective lens: use lensless coherent electron diffraction imaging, do not use the objective lens (that is, the defocusing electromagnetic lens), and shorten the electron flight distance.

3.      解决通过采用兆电子伏特电子脉冲提高时间分辨率的高成本问题:采用无透镜相干电子衍射成像,不使用物镜,大幅度降低成本。 3. Solve the high-cost problem of improving time resolution by using megaelectron-volt electron pulses: use lensless coherent electron diffraction imaging, without using an objective lens, and greatly reduce costs.

4.      实现超高空间分辨率:由于采用高亮度的相干电子束(空间相干长度优于50纳米,时间相干长度优于50纳米)和紧聚焦电子光学(聚焦电子斑小于50纳米),保证电子散射相位的反演,从而使该技术可实现优于1纳米的空间分辨率。 4. Achieve ultra-high spatial resolution: Due to the use of high-brightness coherent electron beams (the spatial coherence length is better than 50 nanometers, and the temporal coherence length is better than 50 nanometers) and tightly focused electron optics (the focused electron spot is less than 50 nanometers), the electron scattering phase is guaranteed The inversion of , so that the technique can achieve a spatial resolution better than 1 nanometer.

5.      实现超高时间分辨率:超快(即时间分辨)电子显微成像可以通过精密调节过程激发脉冲与探测电子脉冲之间的时间延迟,进而探测每一个相对时刻的无透镜相干电子衍射图样,并进行该时刻的反演和样品的三维重构,最终获得泵浦激发样品区域前后的瞬态结构信息。通过控制过程激发脉冲、探测电子脉冲宽度以及两者之间的同步精度均在1皮秒以下,可以实现优于1皮秒的时间分辨率。 5. Achieve ultra-high time resolution: Ultrafast (i.e., time-resolved) electron microscopy imaging can detect the lensless coherent electron diffraction pattern at each relative moment by precisely adjusting the time delay between the process excitation pulse and the detection electron pulse, and The inversion at this moment and the three-dimensional reconstruction of the sample are carried out to finally obtain the transient structure information before and after the pump excites the sample region. Time resolution better than 1 picosecond can be achieved by controlling the process excitation pulse, the probe electron pulse width, and the synchronization between the two with an accuracy of less than 1 picosecond.

与现有技术相比,本发明的有益效果是: Compared with prior art, the beneficial effect of the present invention is:

1.实现超高时间分辨和超高空间分辨的瞬态成像:它利用了与过程激发源(如激光)精确同步的高能电子脉冲,结合泵浦-探测方法,可同时实现超高时间分辨(优于1皮秒)和超高空间分辨(优于1纳米)的瞬态成像能力。 1. Transient imaging with ultra-high time resolution and ultra-high spatial resolution: it utilizes high-energy electron pulses precisely synchronized with process excitation sources (such as lasers), combined with pump-probe methods, and can simultaneously achieve ultra-high time resolution (better than 1 picosecond) and ultra-high spatial resolution (better than 1 nanometer) transient imaging capabilities.

2.避免电磁透镜对提高时间分辨率的限制:它的无透镜设计,避免了飞秒探测电子脉冲经过电子透镜后的脉冲展宽,保持了电子脉冲宽度,保证了该方法的时间分辨率。 2. Avoid the limitation of electromagnetic lens to improve the time resolution: its lensless design avoids the pulse broadening of the femtosecond detection electron pulse after passing through the electron lens, maintains the electron pulse width, and ensures the time resolution of the method.

3.极大降低成本:它的无透镜设计,结构简单,避免采用昂贵的散焦电磁透镜。 3. Greatly reduce costs: Its lensless design, simple structure, avoids the use of expensive defocusing electromagnetic lenses.

4.提供时间分辨电子衍射所缺乏的重要的局域瞬态结构信息。 4. Provides important local transient structural information that time-resolved electron diffraction lacks.

附图说明 Description of drawings

图1是本发明超快无透镜相干电子衍射成像装置的结构简图。 Fig. 1 is a schematic diagram of the structure of the ultrafast lensless coherent electron diffraction imaging device of the present invention.

图2是本发明装置的一个实施例的结构示意图。 Fig. 2 is a schematic structural view of an embodiment of the device of the present invention.

具体实施方式 Detailed ways

下面结合实施例和附图对本发明作进一步说明,但不应以此限制本发明的保护范围。 The present invention will be further described below in conjunction with the embodiments and accompanying drawings, but the protection scope of the present invention should not be limited thereby.

本发明所述的超快无透镜相干电子衍射成像方法具有脉冲电子控制系统简单、空间分辨率不受散焦物镜制约等优点,只需要一组强聚焦磁透镜将脉冲电子聚焦在样品上,无需散焦电磁透镜,就可实现在实空间的超高时间和超高空间分辨。该方法极易与兆电子伏特超快电子衍射相结合,但这一方法对脉冲电子束的相干性有极高的要求。脉冲电子束的相干性以及聚焦电子斑大小决定本发明的空间分辨率。 The ultra-fast lensless coherent electron diffraction imaging method of the present invention has the advantages of simple pulse electronic control system, and the spatial resolution is not restricted by the defocusing objective lens. It only needs a set of strong focusing magnetic lenses to focus the pulse electrons on the sample, without By defocusing the electromagnetic lens, ultra-high time and ultra-high spatial resolution in real space can be realized. This method is very easy to combine with MeV ultrafast electron diffraction, but this method has extremely high requirements on the coherence of the pulsed electron beam. The coherence of the pulsed electron beam and the focused electron spot size determine the spatial resolution of the present invention.

本发明所述的超快无透镜相干电子衍射成像方法所采用的电子脉冲是与过程激发源精确同步;探测电子脉冲的脉冲宽度、过程激发脉冲的脉冲宽度、电子脉冲与过程激发源的同步精度等决定了该方法的时间分辨能力,可以实现1皮秒甚至更优的时间分辨率。 The electronic pulse used in the ultrafast lensless coherent electron diffraction imaging method of the present invention is precisely synchronized with the process excitation source; the pulse width of the detection electronic pulse, the pulse width of the process excitation pulse, and the synchronization accuracy of the electronic pulse and the process excitation source etc. determine the time resolution capability of the method, and a time resolution of 1 picosecond or even better can be achieved.

先请参阅图1,图1是本发明超快无透镜相干电子衍射成像装置的结构简图。本发明超快无透镜相干电子衍射成像装置,由过程激发源01、脉冲电子系统02、脉冲电子控制系统03、样品04、探测系统05、数据处理和三维重构系统06和高真空样品靶室07组成,上述元部件的功能和位置关系如下: Please refer to FIG. 1 first. FIG. 1 is a schematic structural diagram of an ultrafast lensless coherent electron diffraction imaging device of the present invention. The ultrafast lensless coherent electron diffraction imaging device of the present invention consists of a process excitation source 01, a pulse electronic system 02, a pulse electronic control system 03, a sample 04, a detection system 05, a data processing and three-dimensional reconstruction system 06 and a high vacuum sample target chamber 07, the functions and positional relationship of the above components are as follows:

所述的脉冲电子系统02、脉冲电子控制系统03、样品04和探测系统05置于所述的高真空样品靶室07,样品04置于高真空样品靶室07内的五维调整架上,其中所述的脉冲电子系统02由脉冲电子源及其加速、整形元件组成;所述的过程激发源01产生过程激发脉冲,输入所述的高真空样品靶室07激发位于所述的五维调整架上的样品04。 The pulse electronic system 02, the pulse electronic control system 03, the sample 04 and the detection system 05 are placed in the high vacuum sample target chamber 07, and the sample 04 is placed on the five-dimensional adjustment frame in the high vacuum sample target chamber 07, The pulsed electron system 02 is composed of a pulsed electron source and its acceleration and shaping components; the process excitation source 01 generates a process excitation pulse, which is input into the high vacuum sample target chamber 07 to excite the five-dimensional adjustment Sample 04 on shelf.

所述的脉冲电子源产生与所述的过程激发脉冲精确同步的电子脉冲,该脉冲电子经过加速、整形成为高亮度相干的脉冲电子束,经过所述的脉冲电子控制系统03聚焦照射在处于高真空样品靶室07内的被过程激发脉冲激发的样品区域,被所述的样品衍射后,形成一系列相互耦合的、或者相互重叠的衍射图样;该衍射图样有所述的探测系统05接收,包括布拉格衍射峰以及布拉格峰间的干涉信息;输入所述的数据处理和三维重构系统06,通过在线快速傅里叶方法,从衍射图样中找回相位。 The pulsed electron source generates electron pulses that are precisely synchronized with the process excitation pulses. The pulsed electrons are accelerated and shaped into high-brightness coherent pulsed electron beams, which are focused and irradiated at a high temperature by the pulsed electronic control system 03 The sample area excited by the process excitation pulse in the vacuum sample target chamber 07 is diffracted by the sample to form a series of mutually coupled or overlapping diffraction patterns; the diffraction patterns are received by the detection system 05, Including Bragg diffraction peaks and interference information between Bragg peaks; input to the data processing and three-dimensional reconstruction system 06, and retrieve the phase from the diffraction pattern through the online fast Fourier method.

请参阅图2,图2是本发明装置的一个实施例的结构示意图。实施例是以飞秒脉冲激光为过程激发源的装置,由图可见,本发明超快无透镜相干电子衍射成像装置的构成: Please refer to FIG. 2 . FIG. 2 is a schematic structural diagram of an embodiment of the device of the present invention. The embodiment is a device with a femtosecond pulsed laser as the process excitation source. As can be seen from the figure, the composition of the ultrafast lensless coherent electron diffraction imaging device of the present invention:

所述的过程激发源01包括飞秒激光光源1、分束镜2、由第一激光伺服反射镜3、第二激光伺服反射镜4和第一平移台5构成的第一可变光路延迟调节系统、第三激光伺服反射镜6、光参量放大激光转化系统7、第四激光伺服反射镜8、聚焦透镜9构成。 The process excitation source 01 includes a femtosecond laser light source 1, a beam splitter 2, a first variable optical path delay adjustment composed of a first laser servo mirror 3, a second laser servo mirror 4 and a first translation stage 5 system, the third laser servo mirror 6, the optical parameter amplification laser transformation system 7, the fourth laser servo mirror 8, and the focusing lens 9.

所述的脉冲电子系统02由位于高真空样品靶室24外的第五激光伺服反射镜10、由第六激光伺服反射镜11、第七激光伺服反射镜12和第二平移台13构成的第二光路延迟调节系统、第八激光伺服反射镜28、飞秒激光三倍频装置14、紫外聚焦透镜15和位于高真空样品靶室24内的金属膜16和多级微波加速器17构成。 The pulsed electronic system 02 is composed of the fifth laser servo mirror 10 located outside the high vacuum sample target chamber 24, the sixth laser servo mirror 11, the seventh laser servo mirror 12 and the second translation stage 13. The second optical path delay adjustment system, the eighth laser servo mirror 28, the femtosecond laser triple frequency device 14, the ultraviolet focusing lens 15, the metal film 16 located in the high vacuum sample target chamber 24 and the multi-stage microwave accelerator 17 are composed.

脉冲电子控制系统03由位于高真空样品靶室24内依次的第一偏转板18、第二偏转板19、由第一电磁透镜20、第一孔径21、第二电磁透镜22、第二孔径23构成。 The pulse electronic control system 03 consists of the first deflection plate 18, the second deflection plate 19, the first electromagnetic lens 20, the first aperture 21, the second electromagnetic lens 22, and the second aperture 23 located in the high vacuum sample target chamber 24. constitute.

沿所述的飞秒激光光源1的激光前进方向是所述的分束镜2,该分束镜2将飞秒激光光源1输出的飞秒激光脉冲分为反射光束A和透射光束B;沿所述的反射光束A的前进方向依次经所述的第一激光伺服反射镜3、第二激光伺服反射镜4、第三激光伺服反射镜6、光参量放大激光转化系统7、第四激光伺服反射镜8反射,经所述的聚焦透镜9聚焦后,穿过所述的高真空样品靶室照射位于五轴样品调节架25上的样品;沿所述的透射光束B的前进方向依次经过所述的第五激光伺服反射镜10、由第六激光伺服反射镜11、第七激光伺服反射镜12、第八激光伺服反射镜28、飞秒激光三倍频装置14和紫外聚焦透镜15聚焦后转化为266nm激光脉冲。 Along the laser advance direction of the femtosecond laser light source 1 is the beam splitter 2, which divides the femtosecond laser pulse output by the femtosecond laser light source 1 into a reflected beam A and a transmitted beam B; The forward direction of the reflected light beam A passes through the first laser servo mirror 3, the second laser servo mirror 4, the third laser servo mirror 6, the optical parameter amplification laser conversion system 7, the fourth laser servo Reflected by the mirror 8, after being focused by the focusing lens 9, the sample located on the five-axis sample adjustment frame 25 is irradiated through the high-vacuum sample target chamber; After the fifth laser servo mirror 10 described above is focused by the sixth laser servo mirror 11, the seventh laser servo mirror 12, the eighth laser servo mirror 28, the femtosecond laser triple frequency device 14 and the ultraviolet focusing lens 15 Converted to 266nm laser pulses.

所述的266nm激光脉冲照射位于所述高真空样品靶室24内的金属膜16上,并通过光电效应产生脉冲电子,该脉冲电子经多级微波加速器17、第一偏转板18、第二偏转板19、由第一电磁透镜20、第一孔径21、第二电磁透镜22、第二孔径23构成的电子聚焦准直系统后照射在所述的样品区域内,被衍射形成的布拉格衍射峰和布拉格峰间干涉信息的衍射图样,该衍射图样由所述的探测系统26接收,送入所述的数据处理和三维重构系统27进行数据处理,利用“位置敏感衍射成像”(PSDI)技术,解析出样品的散射相位信息。 The 266nm laser pulse irradiates the metal film 16 located in the high-vacuum sample target chamber 24, and generates pulsed electrons through the photoelectric effect, and the pulsed electrons are deflected by the multistage microwave accelerator 17, the first deflection plate 18, and the second deflection plate. The plate 19, the electronic focusing and collimation system composed of the first electromagnetic lens 20, the first aperture 21, the second electromagnetic lens 22, and the second aperture 23 are then irradiated in the sample area, and the Bragg diffraction peaks formed by diffraction and Diffraction pattern of Bragg inter-peak interference information, the diffraction pattern is received by the detection system 26, sent to the data processing and three-dimensional reconstruction system 27 for data processing, using the "position-sensitive diffraction imaging" (PSDI) technology, Analyze the scattering phase information of the sample.

所述的过程激发脉冲和所述的电子脉冲通过泵浦-探测技术精确同步。 The process excitation pulses and the electron pulses are precisely synchronized by pump-probe technology.

所述的五轴样品调节架具有上下、前后、左右、旋转和倾斜调整姿态。 The five-axis sample adjustment rack has up and down, front and rear, left and right, rotation and tilt adjustment postures.

所述的第一激光伺服反射镜3和第二激光伺服反射镜4设置于第一平移台5上构成的第一可变光路延迟调节系统,所述的第六激光伺服反射镜11和第七激光伺服反射镜12设置于第二平移台13上构成的第二光路延迟调节系统。 The first variable optical path delay adjustment system formed by the first laser servo mirror 3 and the second laser servo mirror 4 being arranged on the first translation stage 5, the sixth laser servo mirror 11 and the seventh laser servo mirror The laser servo mirror 12 is arranged on the second translation stage 13 to form a second optical path delay adjustment system.

其中放置样品的高真空样品靶室、脉冲电子源的腔室、脉冲电子控制系统的腔室以及探测系统的腔室都处于高真空或超高真空环境,可以通过前级机械泵以及分子泵抽至10-7Pa以下,再通过离子泵及升华泵保持超高真空状态。 Among them, the high-vacuum sample target chamber where the sample is placed, the chamber of the pulsed electron source, the chamber of the pulsed electronic control system, and the chamber of the detection system are all in a high-vacuum or ultra-high-vacuum environment, which can be pumped by the front-stage mechanical pump and molecular pump. to below 10 -7 Pa, and then maintain an ultra-high vacuum state through an ion pump and a sublimation pump.

本发明所述的超快(即时间分辨的)无透镜相干电子衍射成像(即电子显微成像)可以通过精密调节第一平移台5或第二平移台13调节泵浦脉冲与探测电子之间的时间延迟,进而探测每一个相对时刻的无透镜相干电子衍射图样,并进行该时刻的反演和样品的三维重构,最终获得泵浦激发样品区域前后的瞬态结构信息。由于过程激发脉冲在飞秒量级,过程激发脉冲与探测电子脉冲同源(可实现精确同步至飞秒量级),只要通过控制探测电子脉冲宽度在1皮秒以下,以及平移台的移动精度优于150微米,就可以实现优于1皮秒的时间分辨率。 The ultra-fast (i.e. time-resolved) lensless coherent electron diffraction imaging (i.e. electron microscopic imaging) described in the present invention can adjust the distance between the pump pulse and the detection electron by precisely adjusting the first translation stage 5 or the second translation stage 13 time delay, and then detect the lensless coherent electron diffraction pattern at each relative time, and carry out the inversion and three-dimensional reconstruction of the sample at this time, and finally obtain the transient structure information before and after the pump excites the sample area. Since the process excitation pulse is at the femtosecond level, the process excitation pulse and the detection electron pulse have the same source (accurate synchronization to the femtosecond level can be achieved), as long as the detection electron pulse width is controlled below 1 picosecond and the movement accuracy of the translation stage Time resolution better than 1 picosecond can be achieved at better than 150 microns.

本发明所述的发生相干衍射的电子脉冲要求具有一定的空间和时间相干性。电子脉冲的空间相干性和时间相干性决定了该方法的可操作性和空间分辨率。基于目前现有的3 MeV超短电子源,空间相干长度可达30纳米,时间相干长度可达0.5纳米,可以满足飞秒电子衍射的需求。为实现超快无透镜相干电子衍射成像,需要进一步对超短兆电子伏特电子脉冲进行优化,使能散从10-3降至10-5从而提高电子的时间相干长度两个数量级,同时降低电子发散角以提高空间相干长度3倍以上,从而通过导入的双聚焦镜及聚焦镜孔径,超快电子束斑可聚焦到30-50纳米,对纳米粒子、超薄样品都可望实现1纳米的空间分辨,从而实现同时获得超高时间分辨和超高空间分辨能力。 The coherently diffracted electron pulses in the present invention require certain spatial and temporal coherence. The spatial and temporal coherence of the electron pulses determines the operability and spatial resolution of the method. Based on the current 3 MeV ultrashort electron source, the spatial coherence length can reach 30 nanometers, and the temporal coherence length can reach 0.5 nanometers, which can meet the requirements of femtosecond electron diffraction. In order to realize ultrafast lensless coherent electron diffraction imaging, it is necessary to further optimize the ultrashort MeV electron pulse, so that the energy dispersion can be reduced from 10 -3 to 10 -5 , thereby increasing the time coherence length of electrons by two orders of magnitude, while reducing the The divergence angle is used to increase the spatial coherence length by more than 3 times, so that through the imported double focusing mirror and the aperture of the focusing mirror, the ultrafast electron beam spot can be focused to 30-50 nanometers, and it is expected to achieve 1 nanometer for nanoparticles and ultra-thin samples. Spatial resolution, so as to achieve ultra-high time resolution and ultra-high spatial resolution at the same time.

Claims (8)

  1. One kind ultrafast without the relevant electronic diffraction formation method of lens, it is characterized in that: the method is in conjunction with the pumping-detection technology with without the relevant electronic diffraction imaging of lens, to realize simultaneously the transient state imaging of ultrahigh time resolution and superelevation spatial discrimination; The method adopts with the relevant electronic impulse of the high brightness of process excitation pulse precise synchronization as detection source; Directly collect relevant electronic diffraction imaging pattern by detection system after surveying electronics process sample, thereby keep the scattering phase information of electronics; The method utilizes existing Inversion Calculation method to calculate the scattering phase information of electronics from described relevant electronic diffraction imaging by data processing and three-dimensional reconfiguration system, realizes structure and the pattern reconstruct of Three dimensional transient atomic scale.
  2. 2. according to claim 1 ultrafast without the relevant electronic diffraction formation method of lens, it is characterized in that adopting the coherent electron beam of high brightness, its Spatially coherent length is better than 50 nanometers, temporal coherent length is better than 50 nanometers, as detection source and tight focused electron optics, guarantee the inverting of electron scattering phase place, thereby make this technology can realize being better than the spatial resolution of 1 nanometer.
  3. 3. according to claim 1 ultrafast without the relevant electronic diffraction formation method of lens, it is characterized in that the ultrashort electronic impulse of employing and process excitation pulse precise synchronization is as detection source; By the control procedure excitation pulse, survey electronic impulse width and synchronization accuracy between the two all below 1 psec, can realize being better than the temporal resolution of 1 psec.
  4. 4. the pulse duration of electronic impulse, the pulse duration of process excitaton source, electronic impulse are the temporal resolutions that synchronization accuracy etc. with the process excitaton source has determined the method.
  5. 5. implement each described ultrafast ultrafast without the relevant electronic diffraction imaging device of lens without the relevant electronic diffraction formation method of lens of claim 1-3, it is characterized in that, this device is comprised of process excitaton source (01), pulsed electron system (02), pulsed electron control system (03), sample (04), detection system (05), data processing and three-dimensional reconfiguration system (06) and high vacuum sample target chamber (07), and function and the position relationship of above-mentioned component are as follows:
    Described pulsed electron system (02), pulsed electron control system (03), sample (04) and detection system (05) place in the described high vacuum sample target chamber (07), sample (04) places five in the high vacuum sample target chamber (07) to tie up on the adjustment racks, described pulsed electron system (02) is comprised of Pulse Electric component and acceleration thereof, reshaping device, described process excitaton source (01) production process excitation pulse is inputted described high vacuum sample target chamber (07) and is excited the sample (04) that is positioned on the described five dimension adjustment racks;
    Described Pulse Electric component produces the electronic impulse with described process excitation pulse precise synchronization, this pulsed electron becomes the relevant pulsed electron beam of high brightness through acceleration, shaping, focusing is radiated at the sample area that is excited by the process excitation pulse that is in the high vacuum sample target chamber (07) through described pulsed electron control system (03), behind described sample diffraction, form a series of that intercouple or overlapped diffraction patterns; This diffraction pattern is received by described detection system (05), comprises the interference information between Bragg diffraction peak and bragg peak; Input described data and process and three-dimensional reconfiguration system (06), by online fast Fourier method, from diffraction pattern, give phase place for change.
  6. 6. according to claim 2 ultrafast without the relevant electronic diffraction imaging device of lens, it is characterized in that described process excitaton source (01) comprises that femtosecond laser light source (1), beam splitter (2), the first changeable optical path that is made of the first laser servo speculum (3), the second laser servo speculum (4) and the first translation stage (5) postpone regulating system, the 3rd laser servo speculum (6), optical parameter amplifying laser conversion system (7), the 4th laser servo speculum (8), condenser lens (9) formation;
    The second optical path delayed regulating system, the 8th laser servo speculum (28), femtosecond laser frequency tripling device (14), ultraviolet condenser lens (15) that described pulsed electron system (02) consists of by the 5th outer laser servo speculum (10) of high vacuum sample target chamber (24), by the 6th laser servo speculum (11), the 7th laser servo speculum (12) and the second translation stage (13), and be positioned at high vacuum sample target chamber (24) metal film (16) and multistage microwave accelerator (17) formation successively;
    Described pulsed electron control system (03) is by being positioned at successively the first deflector (18) of high vacuum sample target chamber (24), the second deflector (19), being made of the first electromagnetic lens (20), the first aperture (21), the second electromagnetic lens (22), the second aperture (23);
    Laser direction of advance along described femtosecond laser light source (1) is described beam splitter (2), and this beam splitter (2) is divided into folded light beam (A) and transmitted light beam (B) with the femto-second laser pulse of femtosecond laser light source (1) output; Direction of advance along described folded light beam (A) reflects through described the first laser servo speculum (3), the second laser servo speculum (4), the 3rd laser servo speculum (6), optical parameter amplifying laser conversion system (7), the 4th laser servo speculum (8) successively, after described condenser lens (9) focuses on, pass described high vacuum sample target chamber and shine the sample that is positioned on the five axle sample adjusting brackets (25); Pass through successively described the 5th laser servo speculum (10), be converted into the 266nm laser pulse after being focused on by the 6th laser servo speculum (11), the 7th laser servo speculum (12), the 8th laser servo speculum (28), femtosecond laser frequency tripling device (14) and ultraviolet condenser lens (15) along the direction of advance of described transmitted light beam (B);
    Described 266nm laser pulses irradiate is positioned on the metal film (16) of described high vacuum sample target chamber (24), and by photoelectric effect generation pulsed electron, this electronic impulse is through multistage microwave accelerator (17), the first deflector (18), the second deflector (19), by the first electromagnetic lens (20), the first aperture (21), the second electromagnetic lens (22), be radiated in the described sample area behind the electron focusing colimated light system that the second aperture (23) consists of, the diffraction pattern of interference information between the Bragg diffraction peak of diffracted formation and bragg peak, this diffraction pattern is received by described detection system (26), send into described data processing and three-dimensional reconfiguration system (27) and carry out the data processing, parse the scattering phase information of sample.
  7. 7. according to claim 3 ultrafastly it is characterized in that without the relevant electronic diffraction imaging device of lens is about described five axle sample adjusting brackets have, all around, rotation and tilt adjustments attitude.
  8. 8. according to claim 3 ultrafast without the relevant electronic diffraction imaging device of lens, it is characterized in that, described the first laser servo speculum (3) and the second laser servo speculum (4) are arranged at upper the first changeable optical path that consists of of the first translation stage (5) and postpone regulating system, and described the 6th laser servo speculum (11) and the 7th laser servo speculum (12) are arranged at upper the second optical path delayed regulating system that consists of of the second translation stage (13).
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CN103175823A (en) * 2013-03-07 2013-06-26 东南大学 Double-delay displacement platform femtosecond laser transient heat reflecting system
CN104766776A (en) * 2014-01-07 2015-07-08 中国科学院物理研究所 Multifunctional Ultrafast Transmission Electron Microscopy Electron Gun
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CN107101974A (en) * 2017-07-03 2017-08-29 西京学院 A kind of new three step is without lens coherent diffraction imaging method
CN109782508A (en) * 2018-12-17 2019-05-21 复旦大学 A kind of method of nonlinear effect amplification and detection electronics ultrafast process
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CN111490437A (en) * 2019-04-15 2020-08-04 中国科学院物理研究所 Device and method for inducing frequency-controllable microwave radiation by the interaction of laser and antenna target
CN111929646A (en) * 2020-08-14 2020-11-13 中国地质大学(北京) Beam scanning ground penetrating radar system and intelligent beam scanning detection method

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